US3899341A - Refractory fired shaped element and process of its manufacture - Google Patents

Refractory fired shaped element and process of its manufacture Download PDF

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Publication number
US3899341A
US3899341A US458022A US45802274A US3899341A US 3899341 A US3899341 A US 3899341A US 458022 A US458022 A US 458022A US 45802274 A US45802274 A US 45802274A US 3899341 A US3899341 A US 3899341A
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United States
Prior art keywords
zirconium oxide
weight
shaped element
zirconium
refractory
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
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US458022A
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English (en)
Inventor
Hans Georg Schwarz
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Didier Werke AG
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Didier Werke AG
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Filing date
Publication date
Priority claimed from DE19732321810 external-priority patent/DE2321810C3/de
Application filed by Didier Werke AG filed Critical Didier Werke AG
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Publication of US3899341A publication Critical patent/US3899341A/en
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Expired - Lifetime legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/48—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates
    • C04B35/481—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates containing silicon, e.g. zircon
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
    • B22D41/00—Casting melt-holding vessels, e.g. ladles, tundishes, cups or the like
    • B22D41/14—Closures
    • B22D41/16—Closures stopper-rod type, i.e. a stopper-rod being positioned downwardly through the vessel and the metal therein, for selective registry with the pouring opening
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
    • B22D41/00—Casting melt-holding vessels, e.g. ladles, tundishes, cups or the like
    • B22D41/50—Pouring-nozzles
    • B22D41/52—Manufacturing or repairing thereof
    • B22D41/54—Manufacturing or repairing thereof characterised by the materials used therefor
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
    • C04B2235/3208—Calcium oxide or oxide-forming salts thereof, e.g. lime
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3244—Zirconium oxides, zirconates, hafnium oxides, hafnates, or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3244—Zirconium oxides, zirconates, hafnium oxides, hafnates, or oxide-forming salts thereof
    • C04B2235/3246—Stabilised zirconias, e.g. YSZ or cerium stabilised zirconia
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3244—Zirconium oxides, zirconates, hafnium oxides, hafnates, or oxide-forming salts thereof
    • C04B2235/3248—Zirconates or hafnates, e.g. zircon
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/50—Constituents or additives of the starting mixture chosen for their shape or used because of their shape or their physical appearance
    • C04B2235/54—Particle size related information
    • C04B2235/5418—Particle size related information expressed by the size of the particles or aggregates thereof
    • C04B2235/5427—Particle size related information expressed by the size of the particles or aggregates thereof millimeter or submillimeter sized, i.e. larger than 0,1 mm
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/50—Constituents or additives of the starting mixture chosen for their shape or used because of their shape or their physical appearance
    • C04B2235/54—Particle size related information
    • C04B2235/5418—Particle size related information expressed by the size of the particles or aggregates thereof
    • C04B2235/5436—Particle size related information expressed by the size of the particles or aggregates thereof micrometer sized, i.e. from 1 to 100 micron
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/60—Aspects relating to the preparation, properties or mechanical treatment of green bodies or pre-forms
    • C04B2235/602—Making the green bodies or pre-forms by moulding
    • C04B2235/6027—Slip casting
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/60—Aspects relating to the preparation, properties or mechanical treatment of green bodies or pre-forms
    • C04B2235/604—Pressing at temperatures other than sintering temperatures
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/74—Physical characteristics
    • C04B2235/77—Density

Definitions

  • the closures are subjected torigorous requirements in regard to the resistance to wear, in relation to the steel, iron or metal flowing the rethrough high temperatures, and particularly in regard; to resistance to deterioration as a result steep changes of temperatures, since the pouring units providedwith the ties of employing nozzles of zirconium silicate are limited.
  • the difficulties associated with zirconium silicate nozzles result during long casting periods and while casting rimmed or alloyed steels.
  • the severe stress manifests itself in the noticeable widening of the cross section of the nozzle opening, which leads to an uncontrolled variation in the rate of pour.
  • Previous attempts to remedy this problem included employment of closures made of zirconium oxide or dense aluminum oxide.
  • wide application of such products is prevented by the price of the material, which is very high in comparison with the products of zirconium silicate, and, most importantly, by a high sensitivity to thermal shock, which is found in such products.
  • the invention is based on the task of developing a reasonably priced, quality zirconium-based material for shaped elements to be inserted into closures in casting units for steel, iron and metal, which encompasses the advantages of a high resistance to wear and to a high resistance in regard to thermal shocks.
  • the problem is solved by employing a composition comprising zirconium oxide at 10 50 by weight, preferably 35 by weight, zirconium silicate at 50 9O by weight, preferably 65 by weight. Moreover,
  • the zirconium oxide is employed in a grain size of at most 0.1 mm, and preferably smaller than 0.06 mm, and the zirconium silicate is introduced in a grain size exceeding 02 mm, preferably 0.2 O.5 mm.
  • zirconium oxide (grain size under 0.1 mm, preferably smaller than 0.06 mm) is based on the idea of introducing this valuable material only in an amount required for a good resistance to corrosion.
  • this corrosion-resistant material forms the matrix, due to its fine grains, which matrix is resistant to slag corrosion.
  • zirconium silicate in H -material, which'is more succep tibleto slag corrosion 20'" then zirconium oxide, is'made si'rnilar to that of zirconium oxide through its employment in theform of coarse grains (0.2 0.5 mm).
  • silicate comprising an intermediate matrix of sintered ""zirc onium oxide. Since the known dissociation of the ZrSiO, at high temperatures zrsio, zro SiO proceeds from the inner surface, the fractionof silicic acid released through decomposition in the composition of the mixtureof the invention (ZrSiO, being in coarser grain) is smaller by a multiple than the fraction corresponding to the quantitative substitution of the ZrSiO in the mixture by ZrO This again leads to the fact that the matrix contains a smaller amount of lowmelting compounds and, consequently, is much more effective against the corrosive action at high temperature. Moreover, the ZrSiO framework confers a good stability in relation to the variation of temperature to the fired product.
  • the shaped elements are manufactured both in accordance with the ceramic slurry casting process and also in accordance with the pressing process. ln order to avoid contamination of the starting material, a zirconium-oxide-containing slurry is used in the casting process. In the pressing process, this slurry or organic binding materials are employed as binders. In order to avoid contamination of the zirconium material through abrasion of foreign substances, the slurry is produced in a wet mill whose lining consists of shaped elements of zirconium oxide, which elements in suitable shape also perform the function of grinding elements.
  • the steel-pouring nozzles produced in accordance with this process possess the following properties:
  • a refractory fired shaped element for closures in casting units for metals comprising 10 to 50 by weight zirconium oxide and 50 to by weight zirconium silicate, 30 to 60 by weight of the total amount of zirconium oxide being present in stabilized form and 70 to 40 by weight of the total amount of zirconium oxide being present in unstabilized form.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Ceramic Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Oxide Ceramics (AREA)
US458022A 1973-04-30 1974-04-04 Refractory fired shaped element and process of its manufacture Expired - Lifetime US3899341A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE19732321810 DE2321810C3 (de) 1973-04-30 Feuerfeste gebrannte Formkörper und Verfahren zu ihrer Herstellung

Publications (1)

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US3899341A true US3899341A (en) 1975-08-12

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US458022A Expired - Lifetime US3899341A (en) 1973-04-30 1974-04-04 Refractory fired shaped element and process of its manufacture

Country Status (10)

Country Link
US (1) US3899341A (fr)
JP (1) JPS5345212B2 (fr)
BE (1) BE813411A (fr)
CA (1) CA1020595A (fr)
ES (1) ES425055A1 (fr)
FR (1) FR2227243B1 (fr)
GB (1) GB1464923A (fr)
IT (1) IT1008467B (fr)
SE (1) SE395880B (fr)
ZA (1) ZA742505B (fr)

Cited By (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4053320A (en) * 1975-06-10 1977-10-11 Keeling & Walker Limited Production of refractory articles
US4513089A (en) * 1980-10-02 1985-04-23 Dynamit Nobel Ag Superrefractory dry ramming material based on zirconium oxide for the lining of induction-type crucible furnaces
US4579829A (en) * 1983-12-13 1986-04-01 Garvie Ronald C Zircon/zirconia refractories
US5034358A (en) * 1989-05-05 1991-07-23 Kaman Sciences Corporation Ceramic material and method for producing the same
US20040102308A1 (en) * 2002-11-06 2004-05-27 Simpson Robert E. Crucible material and crucible
US20090111679A1 (en) * 2007-10-31 2009-04-30 Yanxia Lu Low creep refractory ceramic and method of making
EP2090554A1 (fr) * 2008-02-18 2009-08-19 Refractory Intellectual Property GmbH & Co. KG Bande de laitier réfractaire
US20100012484A1 (en) * 2006-12-21 2010-01-21 Saint-Gobain Centre De Recherches Et D'etudes Doped sintered product based on zircon and zirconia
US20100028665A1 (en) * 2007-10-26 2010-02-04 Yanxia Lu Low-creep zircon material with nano-additives and method of making same
US20100089098A1 (en) * 2006-10-16 2010-04-15 Saint-Gobain Centre De Recherches Et D'etudes Europeen SINTERED AND DOPED PRODUCT BASED ON ZIRCON + Nb2O5 or Ta2O5
CN102007089A (zh) * 2008-04-15 2011-04-06 法商圣高拜欧洲实验及研究中心 由基于锆石的填料生产的烧结制品
US11634363B2 (en) 2020-12-29 2023-04-25 Saint-Gobain Ceramics & Plastics, Inc. Refractory object and method of forming

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS584992A (ja) * 1981-07-01 1983-01-12 Hitachi Ltd 磁気電気変換素子
US4791978A (en) * 1987-11-25 1988-12-20 Vesuvius Crucible Company Gas permeable stopper rod

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2553265A (en) * 1947-11-06 1951-05-15 Corning Glass Works Method of making zircon refractory
US2593352A (en) * 1945-08-23 1952-04-15 Shaw Production of zirconium silicate refractory
US2624097A (en) * 1951-01-09 1953-01-06 Norton Co Method of making dense, hard, abrasion resistant ceramic articles
US3175919A (en) * 1962-06-06 1965-03-30 Harbison Walker Refractories Zirconia refractory
US3228778A (en) * 1964-04-08 1966-01-11 Harbison Walker Refractories Glass furnace lining
US3620781A (en) * 1969-08-06 1971-11-16 Corning Glass Works Partially stabilized zirconia refractory

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2593352A (en) * 1945-08-23 1952-04-15 Shaw Production of zirconium silicate refractory
US2553265A (en) * 1947-11-06 1951-05-15 Corning Glass Works Method of making zircon refractory
US2624097A (en) * 1951-01-09 1953-01-06 Norton Co Method of making dense, hard, abrasion resistant ceramic articles
US3175919A (en) * 1962-06-06 1965-03-30 Harbison Walker Refractories Zirconia refractory
US3228778A (en) * 1964-04-08 1966-01-11 Harbison Walker Refractories Glass furnace lining
US3620781A (en) * 1969-08-06 1971-11-16 Corning Glass Works Partially stabilized zirconia refractory

Cited By (23)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4053320A (en) * 1975-06-10 1977-10-11 Keeling & Walker Limited Production of refractory articles
US4513089A (en) * 1980-10-02 1985-04-23 Dynamit Nobel Ag Superrefractory dry ramming material based on zirconium oxide for the lining of induction-type crucible furnaces
US4579829A (en) * 1983-12-13 1986-04-01 Garvie Ronald C Zircon/zirconia refractories
US5034358A (en) * 1989-05-05 1991-07-23 Kaman Sciences Corporation Ceramic material and method for producing the same
US20040102308A1 (en) * 2002-11-06 2004-05-27 Simpson Robert E. Crucible material and crucible
US8236719B2 (en) 2006-10-16 2012-08-07 Saint-Gobain Centre De Recherches Et D'etudes European Sintered and doped product based on zircon + Nb2O5 or Ta2O5
JP2012236766A (ja) * 2006-10-16 2012-12-06 Saint-Gobain Centre De Recherches & D'etudes Europeen ジルコン＋Ｎｂ２Ｏ５またはＴａ２Ｏ５ベースの焼成及びドープ生成物
US20100089098A1 (en) * 2006-10-16 2010-04-15 Saint-Gobain Centre De Recherches Et D'etudes Europeen SINTERED AND DOPED PRODUCT BASED ON ZIRCON + Nb2O5 or Ta2O5
JP2011502918A (ja) * 2006-10-16 2011-01-27 サン−ゴベン・セントル・ドゥ・レシェルシェ・エ・デチュード・ユーロペアン ジルコン＋Ｎｂ２Ｏ５またはＴａ２Ｏ５ベースの焼成及びドープ生成物
US9573850B2 (en) 2006-12-21 2017-02-21 Saint-Gobain Centre De Recherches Et D'etudes Europeen Doped sintered product based on zircon and zirconia
US20100012484A1 (en) * 2006-12-21 2010-01-21 Saint-Gobain Centre De Recherches Et D'etudes Doped sintered product based on zircon and zirconia
US20100028665A1 (en) * 2007-10-26 2010-02-04 Yanxia Lu Low-creep zircon material with nano-additives and method of making same
US20090111679A1 (en) * 2007-10-31 2009-04-30 Yanxia Lu Low creep refractory ceramic and method of making
US8986597B2 (en) 2007-10-31 2015-03-24 Corning Incorporated Low creep refractory ceramic and method of making
EA017317B1 (ru) * 2008-02-18 2012-11-30 Рефректори Интеллекчуал Проперти Гмбх Унд Ко Кг Огнеупорное изделие для разливочного ковша в виде защитной трубы, запорного стержня, погружного разливочного стакана или погружной разливочной трубы
WO2009103949A1 (fr) * 2008-02-18 2009-08-27 Refractory Intellectual Property Gmbh & Co Kg Bande de laitier réfractaire
US8809214B2 (en) 2008-02-18 2014-08-19 Refractory Intellectual Property Gmbh & Co. Kg Refractory slag band
EP2090554A1 (fr) * 2008-02-18 2009-08-19 Refractory Intellectual Property GmbH & Co. KG Bande de laitier réfractaire
US20110107796A1 (en) * 2008-04-15 2011-05-12 Saint-Gobain Centre De Recherches Et D'etudes Europeen Sintered product produced from a zircon-based charge
CN102007089A (zh) * 2008-04-15 2011-04-06 法商圣高拜欧洲实验及研究中心 由基于锆石的填料生产的烧结制品
US8258068B2 (en) 2008-04-15 2012-09-04 Saint-Gobain Centre De Recherches Et D'etudes Europeen Sintered product produced from a zircon-based charge
CN102007089B (zh) * 2008-04-15 2013-11-13 法商圣高拜欧洲实验及研究中心 由基于锆石的填料生产的烧结制品
US11634363B2 (en) 2020-12-29 2023-04-25 Saint-Gobain Ceramics & Plastics, Inc. Refractory object and method of forming

Also Published As

Publication number Publication date
SE395880B (sv) 1977-08-29
GB1464923A (en) 1977-02-16
JPS5026814A (fr) 1975-03-19
BE813411A (fr) 1974-07-31
CA1020595A (en) 1977-11-08
FR2227243A1 (fr) 1974-11-22
FR2227243B1 (fr) 1978-08-04
IT1008467B (it) 1976-11-10
ES425055A1 (es) 1976-11-16
JPS5345212B2 (fr) 1978-12-05
ZA742505B (en) 1975-04-30
DE2321810A1 (de) 1974-11-14
DE2321810B2 (de) 1976-05-20

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